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Self-doped Conjugated Polyelectrolytes for Bioelectronics Applications
Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Self-doped conjugated polyelectrolytes (CPEs) are a class of conducting polymers constituted of a π-conjugated backbone and charged side groups. The ionic groups provide the counterions needed to balance the charged species formed in the CPEs backbones upon oxidation. As a result, addition of external counterions is not required, and the CPEs can be defined as selfdoped. The combination of their unique optical and electrical properties render them the perfect candidates for optoelectronic applications. Additionally, their “soft” nature provide for the mechanical compatibility necessary to interface with biological systems, rendering them promising materials for bioelectronics applications. CPEs solubility, aggregation state, and optoelectronic properties can be easily tuned by different means, such as blending or interaction with oppositely charged species (such as surfactants), in order to produce materials with the desired properties. In this thesis both the strategies have been explored to produce new functional materials that can be deposited to form a thin film and,  therefore, used as an active layer in organic electrochemical transistors (OECTs). Microstructure formation of the films as well as influence on devices operation and performance have been investigated. We also show that these methods can be exploited to produce materials whose uniquecombination of self-doping ability and hydrophobicity allows incorporation into the phospholipid double layer of biomembranes, while retaining their properties. As a result, self-doped CPEs can be used both as sensing elements to probe the physical state of biomembranes, and as functional ones providing them with new functionalities, such as electrical conductivity. Integration of conductive electronic biomembranes into OECTs devices has brought us one step forward on the interface of manmade technologies with biological systems.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2016. , 68 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1802
National Category
Materials Chemistry Textile, Rubber and Polymeric Materials Inorganic Chemistry Other Materials Engineering Polymer Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-132731DOI: 10.3384/diss.diva-132731ISBN: 9789176856451 (Print)OAI: oai:DiVA.org:liu-132731DiVA: diva2:1048490
Public defence
2016-12-15, Plank, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2016-11-21 Created: 2016-11-21 Last updated: 2016-11-21Bibliographically approved
List of papers
1. Conjugated Polyelectrolyte Blends for Electrochromic and Electrochemical Transistor Devices
Open this publication in new window or tab >>Conjugated Polyelectrolyte Blends for Electrochromic and Electrochemical Transistor Devices
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2015 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 27, no 18, 6385-6393 p.Article in journal (Refereed) Published
Abstract [en]

Two self-doped conjugated polyelectrolytes, having semiconducting and metallic behaviors, respectively, have been blended from aqueous solutions in order to produce materials with enhanced optical and electrical properties. The intimate blend of two anionic conjugated polyelectrolytes combine the electrical and optical properties of these, and can be tuned by blend stoichiometry. In situ conductance measurements have been done during doping of the blends, while UV vis and EPR spectroelectrochemistry allowed the study of the nature of the involved redox species. We have constructed an accumulation/depletion mode organic electrochemical transistor whose characteristics can be tuned by balancing the stoichiometry of the active material.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2015
National Category
Materials Chemistry Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-122212 (URN)10.1021/acs.chemmater.5b02501 (DOI)000361935000028 ()
Note

Funding Agencies|Marie Curie network "Renaissance"; Knut and Alice Wallenberg foundation through Wallenberg Scholar grant; Swedish Research Council [VR-2014-3079, D0556101]; Carl Trygger Foundation [CTS 12:206]

Available from: 2015-10-26 Created: 2015-10-23 Last updated: 2016-11-21
2. Electronic polymers in lipid membranes
Open this publication in new window or tab >>Electronic polymers in lipid membranes
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2015 (English)In: Scientific Reports, ISSN 2045-2322, Vol. 5, no 11242Article in journal (Refereed) Published
Abstract [en]

Electrical interfaces between biological cells and man-made electrical devices exist in many forms, but it remains a challenge to bridge the different mechanical and chemical environments of electronic conductors (metals, semiconductors) and biosystems. Here we demonstrate soft electrical interfaces, by integrating the metallic polymer PEDOT-S into lipid membranes. By preparing complexes between alkyl-ammonium salts and PEDOT-S we were able to integrate PEDOT-S into both liposomes and in lipid bilayers on solid surfaces. This is a step towards efficient electronic conduction within lipid membranes. We also demonstrate that the PEDOT-S@alkyl-ammonium: lipid hybrid structures created in this work affect ion channels in the membrane of Xenopus oocytes, which shows the possibility to access and control cell membrane structures with conductive polyelectrolytes.

Place, publisher, year, edition, pages
Nature Publishing Group, 2015
National Category
Biophysics
Identifiers
urn:nbn:se:liu:diva-120045 (URN)10.1038/srep11242 (DOI)000356090400002 ()26059023 (PubMedID)
Note

Funding Agencies|Knut and Alice Wallenberg Foundation; Swedish Research Council

Available from: 2015-07-06 Created: 2015-07-06 Last updated: 2016-11-21
3. Conjugated Polyelectrolyte Blend as Photonic Probe of Biomembrane Organization
Open this publication in new window or tab >>Conjugated Polyelectrolyte Blend as Photonic Probe of Biomembrane Organization
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2016 (English)In: ChemistrySelect, ISSN 2365-6549, Vol. 1, no 14, 4340-4344 p.Article in journal (Refereed) Published
Abstract [en]

In the following report, a conjugated polyelectrolyte (CPE) blend has been introduced for the first time as a fluorescent probe of membrane organization. Insertion of the blend into the lipid double layer has been rendered possible through formation of a hydrophobic complex by counterion exchange. Changes in membrane physical state from liquid-disordered (Ldis) to liquid-ordered (Lord), and to solid-ordered (Sord) result in red shifts of blend excitation (up to Δλex=+90 nm) and emission (up to Δλnm=+37 nm) maxima attributable to backbone planarization of CPEs. We found that blend stoichiometry can be adjusted to attain the best interplay among single polyelectrolytes properties, such as sensitivity and luminescence. The resulting probes therefore allow a bimodal detection of membrane physical state: changes in absorption permit a direct visualization of membrane organization, while variations in emission spectra demonstrate that CPE-blends are a promising probes that can be used for imaging applications.

Place, publisher, year, edition, pages
John Wiley & Sons, 2016
Keyword
Conjugated Polyelectrolytes, Fluorescent Probes, Liposomes, Membrane Probes, Polyelectrolytes blend
National Category
Biomaterials Science Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-132729 (URN)10.1002/slct.201600920 (DOI)
Available from: 2016-11-21 Created: 2016-11-21 Last updated: 2016-11-21Bibliographically approved

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